Rodica Lindenmaier

Four corners: The largest US methane anomaly viewed from space

Methane (CH4) is a potent greenhouse gas and ozone precursor. Quantifying methane emissions is critical for projecting and mitigating changes to climate and air quality. Here we present CH4 observations made from space combined with Earth-based remote sensing column measurements. Results indicate the largest anomalous CH4 levels viewable from space over the conterminous U.S. are located at the Four Corners region in the Southwest U.S. Emissions exceeding inventory estimates, totaling 0.59 Tg CH4/yr [0.50–0.67; 2σ], are necessary to bring high-resolution simulations and observations into agreement. This underestimated source approaches 10% of the EPA estimate of total U.S. CH4 emissions from natural gas. The persistence of this CH4 signal from 2003 onward indicates that the source is likely from established gas, coal, and coalbed methane mining and processing. This work demonstrates that space-based observations can identify anomalous CH4 emission source regions and quantify their emissions with the use of a transport model.

A New Bruker IFS 125HR FTIR Spectrometer for the Polar Environment Atmospheric Research Laboratory at Eureka, Nunavut, Canada: Measurements and Comparison with the Existing Bomem DA8 Spectrometer

Abstract A new Bruker IFS 125HR Fourier transform spectrometer has been installed at the Polar Environment Atmospheric Research Laboratory at Eureka, Nunavut, Canada (80.05°N, 86.42°W). This instrument will become the Network for the Detection of Atmospheric Composition Change’s (NDACC’s) primary instrument at Eureka, replacing the existing Bomem DA8 Fourier transform spectrometer, and will operate throughout the sunlit parts of the year. This paper introduces the new instrument and describes the retrieval procedure, including a comprehensive error analysis. Total columns of O3, HCl, HF, HNO3, N2O, CH4, and CO are presented for the first full year of measurements (2007). Perturbations in the total column resulting from the presence of the Arctic polar vortex over Eureka and the chemical processes within it are visible, as are annual cycles driven by photochemistry and dynamics. Enhancements in the CO total column resulting from specific biomass burning smoke events can also be seen. An intercomparison bet...

Multiscale observations of CO2, 13CO2, and pollutants at Four Corners for emission verification and attribution

Significance Climate change and air pollution caused by fossil-energy-related CO2 and NOx emissions is a capstone societal issue. A critical barrier to an international treaty aimed toward controlling emissions is the inability to verify inventories and reduction of emissions claimed by individual nations following implementation of new technologies. We demonstrate for the first time, to our knowledge, that simultaneous remote observations of CO2, NO2, and CO regional column enhancements can be made with high fidelity and frequency. These can then be used to identify emissions from power plants and to distinguish them from other sources. Our findings represent a significant advancement in remote sensing monitoring methodology and can be used to develop an enforceable, transparent, and equitable climate treaty. There is a pressing need to verify air pollutant and greenhouse gas emissions from anthropogenic fossil energy sources to enforce current and future regulations. We demonstrate the feasibility of using simultaneous remote sensing observations of column abundances of CO2, CO, and NO2 to inform and verify emission inventories. We report, to our knowledge, the first ever simultaneous column enhancements in CO2 (3–10 ppm) and NO2 (1–3 Dobson Units), and evidence of δ13CO2 depletion in an urban region with two large coal-fired power plants with distinct scrubbing technologies that have resulted in ∆NOx/∆CO2 emission ratios that differ by a factor of two. Ground-based total atmospheric column trace gas abundances change synchronously and correlate well with simultaneous in situ point measurements during plume interceptions. Emission ratios of ∆NOx/∆CO2 and ∆SO2/∆CO2 derived from in situ atmospheric observations agree with those reported by in-stack monitors. Forward simulations using in-stack emissions agree with remote column CO2 and NO2 plume observations after fine scale adjustments. Both observed and simulated column ∆NO2/∆CO2 ratios indicate that a large fraction (70–75%) of the region is polluted. We demonstrate that the column emission ratios of ∆NO2/∆CO2 can resolve changes from day-to-day variation in sources with distinct emission factors (clean and dirty power plants, urban, and fires). We apportion these sources by using NO2, SO2, and CO as signatures. Our high-frequency remote sensing observations of CO2 and coemitted pollutants offer promise for the verification of power plant emission factors and abatement technologies from ground and space.

Global land mapping of satellite-observed CO2 total columns using spatio-temporal geostatistics

ABSTRACT This study presents an approach for generating a global land mapping dataset of the satellite measurements of CO2 total column (XCO2) using spatio-temporal geostatistics, which makes full use of the joint spatial and temporal dependencies between observations. The mapping approach considers the latitude-zonal seasonal cycles and spatio-temporal correlation structure of XCO2, and obtains global land maps of XCO2, with a spatial grid resolution of 1° latitude by 1° longitude and temporal resolution of 3 days. We evaluate the accuracy and uncertainty of the mapping dataset in the following three ways: (1) in cross-validation, the mapping approach results in a high correlation coefficient of 0.94 between the predictions and observations, (2) in comparison with ground truth provided by the Total Carbon Column Observing Network (TCCON), the predicted XCO2 time series and those from TCCON sites are in good agreement, with an overall bias of 0.01 ppm and a standard deviation of the difference of 1.22 ppm and (3) in comparison with model simulations, the spatio-temporal variability of XCO2 between the mapping dataset and simulations from the CT2013 and GEOS-Chem are generally consistent. The generated mapping XCO2 data in this study provides a new global geospatial dataset in global understanding of greenhouse gases dynamics and global warming.

Multi-year comparisons of ground-based and space-borne Fourier Transform Spectrometers in the high Arctic between 2006 and 2013

This paper presents 8 years (2006–2013) of measurements obtained from Fourier transform spectrometers (FTSs) in the high Arctic at the Polar Environment Atmospheric Research Laboratory (PEARL; 80.05 N, 86.42W). These measurements were taken as part of the Canadian Arctic ACE (Atmospheric Chemistry Experiment) validation campaigns that have been carried out since 2004 during the polar sunrise period (from mid-February to mid-April). Each spring, two ground-based FTSs were used to measure total and partial columns of HF, O3, and trace gases that impact O3 depletion, namely, HCl and HNO3. Additionally, some tropospheric greenhouse gases and pollutant species were measured, namely CH4, N2O, CO, and C2H6. During the same time period, the satellite-based ACE-FTS made measurements near Eureka and provided profiles of the same trace gases. Comparisons have been carried out between the measurements from the Portable Atmospheric Research Interferometric Spectrometer for the InfraRed (PARIS-IR) and the co-located high-resolution Bruker 125HR FTS, as well as with the latest version of the ACE-FTS retrievals (v3.5). The total column comparison between the two colocated ground-based FTSs, PARIS-IR and Bruker 125HR, found very good agreement for most of these species (except HF), with differences well below the estimated uncertainties (≤ 6%) and with high correlations (R ≥ 0.8). Partial columns have been used for the ground-based to space-borne comparison, with coincident measurements selected based on time, distance, and scaled potential vorticity (sPV). The comparisons of the ground-based measurements with ACEFTS show good agreement in the partial columns for most species within 6 % (except for C2H6 and PARIS-IR HF), which is consistent with the total retrieval uncertainty of the ground-based instruments. The correlation coefficients (R) of the partial column comparisons for all eight species range from approximately 0.75 to 0.95. The comparisons show no notable increases of the mean differences over these 8 years, indicating the consistency of these datasets and suggesting that the space-borne ACE-FTS measurements have been stable over this period. In addition, changes in the amounts of these trace gases during springtime between 2006 and 2013 are presented and discussed. Increased O3 (0.9%yr−1), HCl (1.7%yr−1), HF (3.8%yr−1), CH4 (0.5 % yr−1), and C2H6 (2.3%yr−1, 2009–2013) have been found with the PARIS-IR dataset, the longer of the two ground-based records. Published by Copernicus Publications on behalf of the European Geosciences Union. 3274 D. Griffin et al.: Ground-based and space-borne FTS comparisons in the high Arctic (2006–2013)

The NOy budget above Eureka, Nunavut from ground-based FTIR measurements, space-based ACE-FTS measurements, and the CMAM-DAS, GEM-BACH, and SLIMCAT models

Reactive nitrogen species, NOy, play an important role in stratospheric chemistry. Using a Bruker 125HR FTIR installed at Eureka, Nunavut, ACE-FTS satellite data, and model simulations, we study the NOy budget for this Arctic site.